Carrier Recombination in Passivated Polycrystalline Perovskite Thin Films

Lead Research Organisation: University of Cambridge
Department Name: Physics

Abstract

Organic-inorganic halide perovskites (OHPs) are the rising stars of photovoltaic and optoelectronic research [1-3]. With power conversion efficiencies surging from 3.8% to 22.7% [4,5] in the last 8 years, OHP solar cells will begin to compete with silicon-based technology in the coming years. However, high defect densities within perovskite materials lead to the parasitic loss of charge carriers via non-radiative recombination (NRR), limiting the efficiencies of state-of-the-art devices. Passivation treatments can be employed to render these defects inert. Such treatments include the chemical doping of perovskite solutions before processing, and the atmospheric post-treatment of films after fabrication [6-9]. The aim of my PhD project is to contribute to a better understanding of the mechanisms that drive NRR in polycrystalline perovskite films, and to uncover the physics behind the passivation treatments which are employed to eliminate defects. Utilising a combination of fast spectroscopy techniques (time-resolved photoluminescence spectroscopy, transient absorption spectroscopy, time-resolved photoemission electron microscopy...) my goal is to characterise the behaviour of carriers under the influence of various passivation methods, to reveal pathways towards more optimal treatments and enhanced device performance. I intend to focus on understanding the role of surface defects - shown to be the most dominant limit on efficiency in OHP thin films [10,11] - using existing surface recombination velocity models [12], as well as through the construction of a comprehensive model of hole-trapping in triple-cation perovskite.

References:
[1] Stranks, S. D. & Snaith, H. J. Metal-halide perovskites for photovoltaic and light-emitting devices. Nature Nanotechnology 10, 391-402 (2015).
[2] Bhatt, M. D. & Lee, J. S. Current progress and scientific challenges in the advancement of organic-inorganic lead halide perovskite solar cells. New Journal of Chemistry 41, 10508-10527 (2017).
[3] Tang, H., He, S. & Peng, C. A Short Progress Report on High-Efficiency Perovskite Solar Cells. Nanoscale Research Letters 12, Article 410 (2017).
[4] Kojima, A., Teshima, K., Shirai, Y. and Miyasaka, T. Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells. J. Am. Chem. Soc. 131, 6050-6051 (2009).
[5] Green, M. A. et al. Solar cell efficiency tables (version 51). Progress in Photovoltaics: Research and Applications 26, 3-12 (2018).
[6] Abdi-Jalebi, M. et al. Maximising and stabilizing luminescence from halide perovskites with potassium passivation. Nature 555, 497-501 (2018).
[7] Tang, Z. et al. Hysterisis-free perovskite solar calls made of potassium-doped organometal halide perovskite. Scientific Reports 7, 12183 (2017).
[8] Zheng, X. et al. Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations. Nature Energy 2, 17102 (2017)
[9] Li, H. et al. Enhancing Efficiency of Perovskite Solar Cells via Surface Passivation with Graphene Oxide Interlayer. ACS Appl. Mater. Interfaces 9, 38967-38976 (2017).
[10] Yang, Y. et al. Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films. Nature Energy 2, Article 16207 (2017).
[11] Zarazua, I. et al. Surface Recombination and Collection Efficiency in Perovskite Solar Cells from Impedance Analysis. J. Phys. Chem. Lett. 7, 5105-5113 (2016).
[12] Yablonovitch, E., Allara, D. L., Chang, C. C., Gmitter, T. & Bright, T. B. Unusually Low Surface-Recombination Velocity on Silicon and Germanium Surfaces. Phys. Rev. Lett. 57, 249-252 (1986).

Publications

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Studentship Projects

Project Reference Relationship Related To Start End Student Name
EP/N509620/1 01/10/2016 30/09/2022
1948691 Studentship EP/N509620/1 01/10/2017 31/03/2021 Stuart Macpherson
 
Description Defects in metal halide perovskites are the limiting factor when it comes to the application of these materials in high-performance solar cell and LED devices. Using a variety of time-resolved spectroscopic and structural tools, the projects funded through this award have helped to elucidate the behaviour of charge carriers in an array of perovskite systems that have been optimised via defect passivation treatments, to improve efficiency and stability.

The work funded by this award has led to important discoveries about charge carrier behaviour in state-of-the-art perovskite materials which could be beneficial for low power LED applications, in the future. The ongoing work has contributed to multiple publications, including one first author journal article.
Exploitation Route There is not yet a complete model or understanding of carrier recombination in perovskite semiconductors. While this funded work is contributing to ongoing material characterisation and develoment of theories, there will remain key questions to answer. What is clear from this award is that nanoscale impurity phases within perovskite semiconductors play a pivotal role in limiting both the performance and stability of these materials, under illumination. This award has helped to distinguish the nature of such phase impurities and has paved a way for addressing them which many aid the overall viability of the technology in the near future.

As the fundamental study of charge carrier behaviour catches up with empirical improvements to solar cell and LED devices, even greater efficiency milestones will become possible.
Sectors Electronics,Energy,Environment

 
Title Research data supporting "Nanoscale Chemical Heterogeneity Dominates the Optoelectronic Response of Alloyed Perovskite Solar Cells" 
Description This repository contains the data required to reproduce the figures from the associated manuscript. This data includes hyperspectral optical imaging cubes, nano X-ray fluorescence and diffraction maps and transient absorption microscopy data. 
Type Of Material Database/Collection of data 
Year Produced 2021 
Provided To Others? Yes  
URL https://www.repository.cam.ac.uk/handle/1810/329908